Organic　scintillators　with　efficient　X-ray　excited　luminescence　are　essential　for　medical　diagnostics　and　security　screening.　However,　achieving　excellent　organic　scintillation　materials　is　challenging　due　to　low　X-ray　absorption　coefficients　and　inferior　radioluminescence　(RL)　intensity.　Herein,　supramolecular　interactions　are　incorporated,　particularly　halogen　bonding,　into　organic　scintillators　to　enhance　their　radioluminescence　properties.　By　introducing　heavy　atoms　(X = Cl,　Br,　I)　into　9,10-bis(4-pyridyl)anthracene　(BPA),　the　formation　of　halogen　bonding　(BPA-X)　enhances　their　X-ray　absorption　coefficient　and　restricts　the　molecular　vibration　and　rotation,　which　boosts　their　RL　intensity.　The　RL　intensity　of　BPA-Cl　and　BPA-Br　fluorochromes　increased　by　over　2　and　6.3　times　compared　to　BPA,　respectively.　Especially,　BPA-Br　exhibits　an　ultrafast　decay　time　of　8.25 ns　and　low　detection　limits　of　25.95 ± 2.49 nGy s−1.　The　flexible　film　constructed　with　BPA-Br　exhibited　excellent　X-ray　imaging　capabilities.　Furthermore,　this　approach　is　also　applicable　to　organic　phosphors.　The　formation　of　halogen　bonding　in　bromophenyl-methylpyridinium　iodide　(PYI)　led　to　a　fourfold　increase　in　RL　intensity　compared　to　bromophenyl-methyl-pyridinium　(PY).　It　suggests　that　halogen　bonding　serves　as　a　promising　and　effective　molecular　design　strategy　for　the　development　of　high-performance　organic　scintillator　materials,　presenting　new　opportunities　for　their　applications　in　radiology　and　security　screening.　©　2023　Wiley-VCH　GmbH.